Nanoscale graphene oxide(NGO)sheets were synthesized and used as carbocatalysts for effectiveoxidation of benzylic alcohols and aromatic aldehydes.For oxidation of alcohols in the presence ofH2O2at80°C,the NGOs(2...Nanoscale graphene oxide(NGO)sheets were synthesized and used as carbocatalysts for effectiveoxidation of benzylic alcohols and aromatic aldehydes.For oxidation of alcohols in the presence ofH2O2at80°C,the NGOs(20%mass fraction)as carbocatalysts showed selectivity toward aldehyde.The rate and yield of this reaction strongly depended on the nature of substituents on the alcohol.For4‐nitrobenzyl alcohol,<10%of it was converted into the corresponding carboxylic acid after24h.By contrast,4‐methoxybenzyl alcohol and diphenylmethanol were completely converted into thecorresponding carboxylic acid and ketone after only9and3h,respectively.The conversion ratesfor oxidation of aromatic aldehydes by NGO carbocatalysts were higher than those for alcohol oxidation.For all the aldehydes,complete conversion to the corresponding carboxylic acids wasachieved using7%(mass fraction)of NGO at70°C within2–3h.Possible mechanisms for NGOcarbocatalyst structure‐dependent oxidation of benzyl alcohols and structure‐independent oxidationof aromatic aldehydes are discussed.展开更多
Lithium-sulfur(Li-S) batteries have the advantages of low-cost and ultra-high energy density(2600 Wh·kg;),which have attracted considerable attention.However,the practical application of Li-S batteries still suff...Lithium-sulfur(Li-S) batteries have the advantages of low-cost and ultra-high energy density(2600 Wh·kg;),which have attracted considerable attention.However,the practical application of Li-S batteries still suffers various intractable problems,such as low electrical conductivity,significant volume expansion,and the shuttle effect of sulfur cathode.Up to now,many tremendous efforts and significant progress have been devoted to settle these problems.One of the most effective strategies is that introducing metal-based compounds(e.g.,metal oxides,-sulfides,-nitrides,carbides,-phosphate,single-metal compounds) to enhance the electrochemical performance of S cathode benefiting from superior adsorption/catalytic ability toward Li;S;(n=1,2,4,8).In this review,we summarized the recent advances in the application of micro/nanoscale catalysts in Li-S system and highlighted the catalytic effect of single-atom compounds.Finally,the challenges and the future research prospects of single-atom catalysts were discussed.展开更多
Combining the advantages of both heterogeneous and homogeneous catalysts,single-atom catalysts(SACs)with unique electronic properties have shown excellent catalytic properties.Herein,we report single-atom Pd dispersed...Combining the advantages of both heterogeneous and homogeneous catalysts,single-atom catalysts(SACs)with unique electronic properties have shown excellent catalytic properties.Herein,we report single-atom Pd dispersed on nanoscale TiO2 prepared by self-assembly method as efficient and selective catalysts for the hydrogenation of phenylacetylene to styrene.The catalysts were characterized by N2 adsorption/desorption,X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and X-ray absorption spectroscopy(XAS).0.2 Pd-TiO2(150℃)possessing dominant single-atom Pd species,exhibited a turnover frequency(TOF)of over 8000 h^-1 with 91%selectivity towards styrene at room temperature.Further increasing Pd loading from 0.2%to 0.5%and 1.5%resulted in the decrease of activity probably due to the formation of Pd nanoparticles.Besides,the 0.2 Pd-TiO2 prepared by self-assembly strategy showed better catalytic performance than commercial 10%Pd/C and0.2 Pd-TiO2 synthesized by using impregnation method.展开更多
By means of chemical reduction,nanoparticles of platinum were deposited on the surface of multi walled carbon nanotubes (MWCNTs).The performance of hydrogen storage of as prepared MWCNTs decorated with platinum was ...By means of chemical reduction,nanoparticles of platinum were deposited on the surface of multi walled carbon nanotubes (MWCNTs).The performance of hydrogen storage of as prepared MWCNTs decorated with platinum was investigated.The results indicate that:(1) Hydrogen uptake is more quick and intense for decorated MWCNTs than that for not decorated ones at 10.931MPa and room temperature.The saturation of hydrogen uptake of the former only lasts about 30min,while the latter needs about 150 min;(2) The amount of hydrogen uptake of decorated MWCNTs is about 1.13wt%, which is larger than that of not decorated ones(about 0.54wt%);(3) However,more than 37% hydrogen absorbed by decorated MWCNTs is chemisorbed.展开更多
The sulfated CeO_(2)/Al_(2)O_(3) catalysts with different sizes of CeO_(2)nanoparticles were prepared by using pure H_2O or acetic acid solution as impregnation solvent, and the influence of sizes of CeO_(2) nanoparti...The sulfated CeO_(2)/Al_(2)O_(3) catalysts with different sizes of CeO_(2)nanoparticles were prepared by using pure H_2O or acetic acid solution as impregnation solvent, and the influence of sizes of CeO_(2) nanoparticles on the catalytic performances of the sulfated CeO_(2)/Al_(2)O_(3) catalyst was studied. The catalytic performance tests show that the sulfated CeO_(2)/Al_(2)O_(3) catalyst using acetic acid solution as impregnation solvent has better catalytic activity and the resistance to K+poisoning than the sulfated CeO_(2)/Al_(2)O_(3) catalyst using pure H_(2)O as impregnation solvent. The excellent catalytic performances can be ascribed to the smaller sizes of CeO_(2) nanoparticles in CeO_(2)/Al_(2)O_(3) catalyst using acetic acid solution, which results in larger amount of adsorbed sulfate species, surface acid sites, surface active oxygen species and excellent redox property. These features are helpful for improving the catalytic performances of sulfated CeO_(2)/Al_(2)O_(3) catalyst using smaller amount of CeO_(2) to cut the costs.展开更多
文摘Nanoscale graphene oxide(NGO)sheets were synthesized and used as carbocatalysts for effectiveoxidation of benzylic alcohols and aromatic aldehydes.For oxidation of alcohols in the presence ofH2O2at80°C,the NGOs(20%mass fraction)as carbocatalysts showed selectivity toward aldehyde.The rate and yield of this reaction strongly depended on the nature of substituents on the alcohol.For4‐nitrobenzyl alcohol,<10%of it was converted into the corresponding carboxylic acid after24h.By contrast,4‐methoxybenzyl alcohol and diphenylmethanol were completely converted into thecorresponding carboxylic acid and ketone after only9and3h,respectively.The conversion ratesfor oxidation of aromatic aldehydes by NGO carbocatalysts were higher than those for alcohol oxidation.For all the aldehydes,complete conversion to the corresponding carboxylic acids wasachieved using7%(mass fraction)of NGO at70°C within2–3h.Possible mechanisms for NGOcarbocatalyst structure‐dependent oxidation of benzyl alcohols and structure‐independent oxidationof aromatic aldehydes are discussed.
基金the National Natural Science Foundation of China(Nos.51771076 and NSFC51621001)Guangdong“Pearl River Talents Plan”(No.2017GC010218)+1 种基金the R&D Program in Key Areas of Guangdong Province(No.2020B0101030005)Guangdong Basic and Applied Basic Research Foundation(No.2020B1515120049)。
文摘Lithium-sulfur(Li-S) batteries have the advantages of low-cost and ultra-high energy density(2600 Wh·kg;),which have attracted considerable attention.However,the practical application of Li-S batteries still suffers various intractable problems,such as low electrical conductivity,significant volume expansion,and the shuttle effect of sulfur cathode.Up to now,many tremendous efforts and significant progress have been devoted to settle these problems.One of the most effective strategies is that introducing metal-based compounds(e.g.,metal oxides,-sulfides,-nitrides,carbides,-phosphate,single-metal compounds) to enhance the electrochemical performance of S cathode benefiting from superior adsorption/catalytic ability toward Li;S;(n=1,2,4,8).In this review,we summarized the recent advances in the application of micro/nanoscale catalysts in Li-S system and highlighted the catalytic effect of single-atom compounds.Finally,the challenges and the future research prospects of single-atom catalysts were discussed.
基金supported by the National University of Singapore Flagship Green Energy Program (#R-279-000-553-646 and R-279-000-553-731)the National Natural Science Foundation of China (21908085)the Natural Science Foundation of Jiangsu Province,China (BK20190961)
文摘Combining the advantages of both heterogeneous and homogeneous catalysts,single-atom catalysts(SACs)with unique electronic properties have shown excellent catalytic properties.Herein,we report single-atom Pd dispersed on nanoscale TiO2 prepared by self-assembly method as efficient and selective catalysts for the hydrogenation of phenylacetylene to styrene.The catalysts were characterized by N2 adsorption/desorption,X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and X-ray absorption spectroscopy(XAS).0.2 Pd-TiO2(150℃)possessing dominant single-atom Pd species,exhibited a turnover frequency(TOF)of over 8000 h^-1 with 91%selectivity towards styrene at room temperature.Further increasing Pd loading from 0.2%to 0.5%and 1.5%resulted in the decrease of activity probably due to the formation of Pd nanoparticles.Besides,the 0.2 Pd-TiO2 prepared by self-assembly strategy showed better catalytic performance than commercial 10%Pd/C and0.2 Pd-TiO2 synthesized by using impregnation method.
文摘By means of chemical reduction,nanoparticles of platinum were deposited on the surface of multi walled carbon nanotubes (MWCNTs).The performance of hydrogen storage of as prepared MWCNTs decorated with platinum was investigated.The results indicate that:(1) Hydrogen uptake is more quick and intense for decorated MWCNTs than that for not decorated ones at 10.931MPa and room temperature.The saturation of hydrogen uptake of the former only lasts about 30min,while the latter needs about 150 min;(2) The amount of hydrogen uptake of decorated MWCNTs is about 1.13wt%, which is larger than that of not decorated ones(about 0.54wt%);(3) However,more than 37% hydrogen absorbed by decorated MWCNTs is chemisorbed.
基金Project supported by the National Natural Science Foundation of China(21607019)the Scientific and Technological Research Program of Chongqing Municipal Education Commission(KJQN202101242,KJQN202001227)the Open Project Program of Key Laboratory of Water Environment Evolution and Pollution Control in the Three Gorges Reservoir(WEPKL2019ZD-04)。
文摘The sulfated CeO_(2)/Al_(2)O_(3) catalysts with different sizes of CeO_(2)nanoparticles were prepared by using pure H_2O or acetic acid solution as impregnation solvent, and the influence of sizes of CeO_(2) nanoparticles on the catalytic performances of the sulfated CeO_(2)/Al_(2)O_(3) catalyst was studied. The catalytic performance tests show that the sulfated CeO_(2)/Al_(2)O_(3) catalyst using acetic acid solution as impregnation solvent has better catalytic activity and the resistance to K+poisoning than the sulfated CeO_(2)/Al_(2)O_(3) catalyst using pure H_(2)O as impregnation solvent. The excellent catalytic performances can be ascribed to the smaller sizes of CeO_(2) nanoparticles in CeO_(2)/Al_(2)O_(3) catalyst using acetic acid solution, which results in larger amount of adsorbed sulfate species, surface acid sites, surface active oxygen species and excellent redox property. These features are helpful for improving the catalytic performances of sulfated CeO_(2)/Al_(2)O_(3) catalyst using smaller amount of CeO_(2) to cut the costs.
